4.8 Article

Precise radiocarbon determination in radioactive waste by a laser-based spectroscopic technique

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NATL ACAD SCIENCES
DOI: 10.1073/pnas.2122122119

关键词

nuclear waste; decommissioning; radiocarbon; nuclear safety; saturated-absorption cavity ring-down spectroscopy

资金

  1. European Commission, Joint Research Centre under the Exploratory Research Programme

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The precise determination of radionuclide inventory in radioactive waste streams is crucial for nuclear waste management. This paper demonstrates the use of laser-based saturated-absorption cavity ring-down (SCAR) spectroscopic technique as an accurate alternative for C-14 content determination in nuclear waste. The results show consistent measurements compared to accelerator mass spectrometry (AMS), indicating the maturity and accuracy of SCAR for C-14 analysis in concrete and graphite samples.
The precise and accurate determination of the radionuclide inventory in radioactive waste streams, including those generated during nuclear decommissioning, is a key aspect in establishing the best-suited nuclear waste management and disposal options. Radiocarbon (C-14) is playing a crucial role in this scenario because it is one of the so-called difficult to measure isotopes; currently, C-14 analysis requires complex systems, such as accelerator mass spectrometry (AMS) or liquid scintillation counting (LSC). AMS has an outstanding limit of detection, but only a few facilities are available worldwide; LSC, which can have similar performance, is more widespread, but sample preparation can be nontrivial. In this paper, we demonstrate that the laser-based saturated-absorption cavity ring-down (SCAR) spectroscopic technique has several distinct advantages and represents a mature and accurate alternative for C-14 content determination in nuclear waste. As a proof-of-principle experiment, we show consistent results of AMS and SCAR for samples of concrete and graphite originating from nuclear installations. In particular, we determined mole fractions of 1.312(9) (FC)-C-14 and 30.951(7) (FC)-C-14 corresponding to similar to 1.5 and 36.2 parts per trillion (ppt), respectively, for two different graphite samples originating from different regions of the Adiabatic Resonance Crossing activator prototype installed on one irradiation line of an MC40 Scanditronix cyclotron. Moreover, we measure a mole fraction of 0.593(8) (FC)-C-14 (similar to 0.7 ppt) from a concrete sample originating from an external wall of the Ispra-1 nuclear research reactor currently in the decommissioning phase.

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